In this chapter, carbon nanofiber (CNF) for hydrogen storage, the pros and cons of use of hydrogen as a source of energy, and various methods of storing hydrogen are presented. Methods of hydrogen storage depend on the state in which it is stored, viz. storage of liquid or gaseous hydrogen. The chapter discusses some of the results of hydrogen storage by different types of carbon nanomaterials. In CNF, graphitic planes are aligned randomly in any orientation relative to the axis of the filament, other than parallel alignment. CNF can also be described in different words, viz. nanofilaments, nanowires and nanofibers. Natural fibers from plants and animals have been converted to graphitic carbon having well-preserved inherent pores by standard carbonization/pyrolytic method, with or without using any catalyst.